发表机构
Solid State and Structural Chemistry Unit; Indian Institute of Science, Bengaluru（固态与结构化学单元; 印度科学研究所）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本文从焓涨落出发，建立脆性与虚拟温度动力学的直接联系，通过焓-焓相关函数统一描述量热弛豫、脆性及非平衡结构停滞。
AI 中文摘要
脆性和虚拟温度是玻璃形成的两个核心度量，但它们的联系通常通过结构弛豫时间或冷却速率依赖性间接表达。本文从构型焓涨落的角度直接阐述这一联系。冷却或老化过程中虚拟温度的时间演化由焓-焓相关函数控制，该函数也决定了频率依赖的构型热容。脆性通过结构弛豫时间的强温度依赖性引入，因此控制着相应的焓弛豫谱在玻璃转变附近向长时间尺度移动的速率。这导致了对虚拟温度滞后产生与增长的直接时域描述，包括德拜极限，并将量热弛豫、脆性和非平衡结构停滞统一在一个共同框架内。
英文摘要
Fragility and fictive temperature are two central measures of glass formation, but their connection is usually expressed indirectly through structural relaxation times or cooling-rate dependence. Here we formulate this connection in terms of configurational enthalpy fluctuations. The time evolution of the fictive temperature during cooling or aging is controlled by the enthalpy--enthalpy correlation function that also determines the frequency-dependent configurational heat capacity. Fragility enters through the strong temperature dependence of the structural relaxation time and therefore controls how rapidly the corresponding enthalpy-relaxation spectrum shifts to long times near the glass transition. This leads to a direct time-domain description of the onset and growth of the fictive-temperature lag, including the Debye limit, and connects calorimetric relaxation, fragility, and nonequilibrium structural arrest within a common framework.
Comments35 pages, 2 Figures
